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Efficient accumulation integrated with selective degradation of micropollutants under irradiation of visible light by the size-exclusion effect of metal–organic framework
Separation and Purification Technology ( IF 8.1 ) Pub Date : 2023-06-07 , DOI: 10.1016/j.seppur.2023.124282
Xin Mi , Xiang Li , Sheng Wang , Chong-Chen Wang , Bo Wang

Developing multifunctional materials for efficiently removing pharmaceutical active compounds (PACs) in water matrix that coexisted with humic acid (HA) is in high demand. Water-stable metal–organic frameworks (MOFs) with tunable porous structures have aroused great attention as versatile adsorbents. However, further eliminating pollutants, especially in practical applications, needs more exploration. In this study, rational modification of UiO-66 (Ce) with a minimum amount of CdS could regulate the highly developed cavities and subsequently promote the selective interfacial degradation of four PACs, including non-steroidal anti-inflammatory drugs and antibiotics with lower concentrations (100 μg/L) detected by HPLC-MS/MS were selected as the model compounds. The adsorption ability of the composites was 11.84 ∼ 12.21 times higher than CdS, and the overall removal efficiency was 1.31 and 2.18 times higher than that of UiO-66 (Ce) and CdS, respectively, via h+ and •O2 generated in simulated HA-containing wastewater. This modification features excellent resistance towards HA (2 mg/L ∼ 10 mg/L) during adsorption and photocatalytic degradation effectively. In comparison, competitive anions (Cl-, SO42-, CO32–, HCO3) with smaller sizes affect ROS formation significantly, indicating the possible exclusion effect of competitors by particular sizes. This study offers a facile strategy to remove PACs and HA-containing water effectively.



中文翻译:

金属-有机骨架尺寸排阻效应在可见光照射下高效积累与选择性降解微污染物

迫切需要开发多功能材料以有效去除水基质中与腐殖酸 (HA) 共存的药物活性化合物 (PAC)。具有可调多孔结构的水稳性金属有机框架(MOF)作为多功能吸附剂引起了人们的极大关注。然而,进一步消除污染物,尤其是在实际应用中,还需要更多的探索。在这项研究中,用最少量的 CdS 对 UiO-66 (Ce) 进行合理修饰可以调节高度发达的空腔,从而促进四种 PAC 的选择性界面降解,包括非甾体抗炎药和较低浓度的抗生素。 100 μg/L)经HPLC-MS/MS检测,被选为模型化合物。复合材料的吸附能力是 CdS 的 11.84 ∼ 12.21 倍,+和 •O 2 产生于模拟的含 HA 废水中。这种修饰在有效吸附和光催化降解过程中对 HA (2 mg/L ∼ 10 mg/L) 具有出色的抵抗力。相比之下,较小尺寸的竞争性阴离子(Cl -、SO 4 2-、CO 3 2–、HCO 3 – )会显着影响 ROS 的形成,表明特定尺寸的竞争者可能存在排斥效应。本研究提供了一种简便的策略来有效去除 PAC 和含 HA 的水。

更新日期:2023-06-09
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